Significance: Owing to potential advantages including ease of use, airtight or watertight sealing, and minimal tissue damage, bioadhesives have been intensively studied and developed as an alternative to sutures and staples to close wounds, achieve hemostasis, and attach and immobilize implantable devices. However, existing bioadhesives have limitations including slow adhesion formation, weak bonding, low biocompatibility, poor mechanical match with tissues, and/or lack of triggerable benign detachment. In this work, we report a bioadhesive capable of instant tough adhesion and triggerable benign detachment that can potentially address all the above-mentioned limitations. The current work not only develops a bioadhesive with superior performances but also advances the understanding of wet adhesion.